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arXiv:1603.02787 · Journal of Physics B Atomic Molecular and Optical Physics

Laser slowing of CaF molecules to near the capture velocity of a molecular MOT

Boerge Hemmerling, Eunmi Chae, Aakash Ravi, Loïc Anderegg, Garrett K Drayna, Nicholas R. Hutzler, Alejandra L Collopy, Jun Ye, Wolfgang Ketterle, John M. Doyle

Published Aug 10, 2016• 94 citations
arXivHTMLPDF

Abstract

Abstract Laser slowing of CaF molecules down to the capture velocity of a magneto-optical trap for molecules is achieved. Starting from a two-stage buffer gas beam source, we apply frequency-broadened ‘white-light’ slowing and observe approximately 6 × 10 4 CaF molecules in a single pulse with velocities 10 ± 4 m s −1 . CaF is a candidate for collisional studies in the mK regime. This work represents a significant step towards magneto-optical trapping of CaF.

DOI
10.1088/0953-4075/49/17/174001

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Laser slowing of CaF molecules down to the capture velocity of a magneto-optical trap for molecules is achieved. Starting from a two-stage buffer gas beam source, we apply frequency-broadened 'white-light' slowing and observe approximately 6 x 10⁴ CaF molecules in a single pulse with velocities 10 ± 4 m s⁻¹. CaF is a candidate for collisional studies in the mK regime. This work represents a significant step towards magneto-optical trapping of CaF.

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Laser Slowing of CaF Molecules and Progress Towards a Dual-MOT for Li and CaF

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arXiv:2610.29033•Oct 21, 2026•0 citations
Abstract Laser slowing of CaF molecules down to the capture velocity of a magneto-optical trap for molecules is achieved. Starting from a two-stage buffer gas beam source, we apply frequency-broadened ‘white-light’ slowing and observe approximately 6 × 10 4 CaF molecules in a single pulse with velocities 10 ± 4 m s −1 . CaF is a candidate for collisional studies in the mK regime. This work represents a significant step towards magneto-optical trapping of CaF.
Diatomic molecules are considered good candidates for the study of strongly correlated systems and precision measurement searches due to their combination of complex internal states and strong long-range interactions. Cooling molecules down to ultracold temperatures is often a necessary step for fully utilizing the power of the molecule. This requires a trap for molecules and the ability to cool molecules to the mK regime and below. A magneto-optical trap (MOT) is a good tool for achieving mK temperatures. However, extra care is needed for molecules to form the necessary quasi-closed cycling transitions due to molecule's complicated energy structure. In our work with CaF, we use two repump lasers to block vibrational leakage and selection rules for the rotational degree of freedom to achieve about 10^{5} photon cycles.\n\n\n\nThe two-stage buffer gas beam source is a general method to generate a cold and slow beam of molecules with a forward velocity of about 50 m/s. The compatibility of the buffer-gas source with a MOT is studied and we confirm that such beams can be nicely compatible with MOTs using various atomic species. \n\n\n\nIn order to load molecules into a MOT from even such a slow beam, additional slowing is required due to the low capture velocity of a molecular MOT (< 10 m/s). We apply a frequency-broadened “white-light” slowing on CaF from a two-stage source, demonstrating slowing of CaF below 10 m/s. An AC MOT, which provides active remixing of dark substates, is also developed and Li atoms are slowed and trapped. These are crucial ingredients for co-trapping CaF molecules and Li atoms and study their collisional properties, which would lead to sympathetic cooling of molecules down to ultracold temperatures. \n\n\n\nThe achievement of slowing and development of this system allowed for the detailed study of the CaF laser cooling system, as well as physical processes involved with AC MOTs and the proposed MOT for CaF. Crucial knowledge of this archetypal system provides significant progress toward manipulation and control of molecules similar to what has been achieved with atoms and what is necessary for searches for new physics with ultracold molecules.
Laser cooling and trapping in a magneto-optical trap (MOT) have been essential to the success of cold atom physics in the last decades. Recently, the application of the same techniques to molecules has begun. The complexity of even a simple diatomic molecule makes laser cooling difficult, but promises new applications in many areas of research. In this thesis I describe the development of the first three-dimensional MOT of calcium fluoride (CaF) molecules. First, a cryogenic buffer gas source was set up, producing a pulsed beam of 9.3*10^10 molecules per steradian per pulse with forward velocities around 170 m/s. A similar source for very large molecules was set up during a 5 month internship at the University of Vienna. Next, the molecular pulse was slowed down to the capture velocity of a MOT using chirped laser slowing, resulting in about 7*10^5 CaF molecules passing through the typical MOT volume of 1 cm^3 at velocities of 15+-5 m/s. A new deceleration method, called Zeeman-Sisyphus deceleration, was also investigated. In this method molecules move through a spatially varying magnetic field and are optically pumped between low- and high-field seeking states in such as a way that they are always losing kinetic energy. The method promises to deliver more slow molecules because the molecules are guided transversely as they are decelerated. A small prototype was built and the optical pumping step was tested successfully. Finally, 7.6*10^3 CaF molecules were trapped in a MOT and cooled to a temperature of 8.5 mK. The radial trap frequency is 2 pi*130 Hz and the damping constant is beta=9.5*10^2 s^-1. The lifetime is about 100 ms and depends strongly on the scattering rate. This MOT is an an ideal starting point for a wide range of new experiments with ultracold molecules.
We present the properties of a magneto-optical trap (MOT) of CaF molecules. We study the process of loading the MOT from a decelerated buffer-gas-cooled beam, and how best to slow this molecular beam in order to capture the most molecules. We determine how the number of molecules, the photon scattering rate, the oscillation frequency, damping constant, temperature, cloud size and lifetime depend on the key parameters of the MOT, especially the intensity and detuning of the main cooling laser. We compare our results to analytical and numerical models, to the properties of standard atomic MOTs, and to MOTs of SrF molecules. We load up to molecules, and measure a maximum scattering rate of s −1 per molecule, a maximum oscillation frequency of 100 Hz, a maximum damping constant of 500 s −1 , and a minimum MOT rms radius of 1.5 mm. A minimum temperature of 730 μ K is obtained by ramping down the laser intensity to low values. The lifetime, typically about 100 ms, is consistent with a leak out of the cooling cycle with a branching ratio of about . The MOT has a capture velocity of about 11 m s −1 .
Using frequency-chirped radiation pressure slowing, we precisely control the velocity of a pulsed CaF molecular beam down to a few m s –1 , compressing its velocity spread by a factor of 10 while retaining high intensity: at a velocity of 15 m s –1 the flux, measured 1.3 m from the source, is 7 × 10 5 molecules per cm 2 per shot in a single rovibrational state. The beam is suitable for loading a magneto-optical trap or, when combined with transverse laser cooling, improving the precision of spectroscopic measurements that test fundamental physics. We compare the frequency-chirped slowing method with the more commonly used frequency-broadened slowing method.
Molecular magneto-optical traps (MOTs) are loaded from cryogenic buffer gas beam (CBGB) sources, which produce a large flux of cold molecules. However, only a small fraction of this flux is slowed and captured. Here, we investigate and optimize one of these CBGB sources through a combination of experiment and simulation to maximize the number of molecules loaded into a MOT of CaF molecules. We experimentally determine the range of molecule velocities from the source that are successfully slowed and captured in the MOT, and perform a systematic study of buffer gas source geometries to identify designs that maximize MOT loading. Our observations agree well with Monte Carlo simulations, which provide physical insight into the dynamics within the source and explain how source geometry influences the subset of molecules that are ultimately trapped. These results provide practical design guidelines for optimizing cryogenic buffer gas beam sources used in laser cooling experiments.